Ultrafast Energy Transfer and Excited State Coupling in an Artificial Photosynthetic Antenna

2013 ◽  
Vol 117 (46) ◽  
pp. 14183-14190 ◽  
Author(s):  
M. Maiuri ◽  
J. J. Snellenburg ◽  
I. H. M. van Stokkum ◽  
S. Pillai ◽  
K. WongCarter ◽  
...  
2002 ◽  
Vol 106 (36) ◽  
pp. 9424-9433 ◽  
Author(s):  
Alisdair N. Macpherson ◽  
Paul A. Liddell ◽  
Darius Kuciauskas ◽  
Dereck Tatman ◽  
Tomas Gillbro ◽  
...  

2008 ◽  
Vol 12 (12) ◽  
pp. 1232-1241 ◽  
Author(s):  
Farid Aziat ◽  
Régis Rein ◽  
Jorge Peón ◽  
Ernesto Rivera ◽  
Nathalie Solladié

In this paper we now report our ongoing progress in the preparation of artificial photosynthetic systems through the preparation of light harvesting multi-porphyrins. A tetramer, constituted of a central dipeptide functionalized by two free-base porphyrins and surrounded by one amino-acid bearing a pendant Zn ( II ) porphyrin on each side, has been chosen. The optical and photophysical properties of this tetramer have been studied by absorption and fluorescence spectroscopy. In addition, the energy transfer phenomenon has been studied and monitored by femtosecond time-resolved fluorescence. Our results indicate that the excited state dynamics redounding in the excitation being localized in the inner free-base porphyrins takes place in the time scale of approximately 1 ps.


2015 ◽  
Vol 19 (01-03) ◽  
pp. 261-269 ◽  
Author(s):  
Mohamed E. El-Khouly ◽  
Cem Göl ◽  
Morad M. El-Hendawy ◽  
Serkan Yeşilot ◽  
Mahmut Durmuş

A molecular pentad, comprised of zinc phthalocyanine ( ZnPc ) with four boron dipyrromethene units (BODIPY) have been examined by femtosecond and nanosecond laser flash photolysis to explore its photoinduced intramolecular events from the excited BODIPY. The geometry optimization showed that the phthalocyanine moiety is completely symmetric and form perfect square planar complex with zinc. The absorption spectrum of ZnPc -BODIPY pentad covers most of the visible region (ca. 300–750 nm), which clearly is an advantage for capturing solar energy. The excitation transfer from the singlet BODIPY to ZnPc is envisioned due to good spectral overlap of the BODIPY emission and ZnPc absorption spectra. Femtosecond laser flash photolysis studies provided concrete evidence for the occurrence of energy transfer from the singlet excited BODIPY to ZnPc in tetrahydrofuran. The kinetic study of energy transfer measured by monitoring the decay of the BODIPY emission revealed fast energy transfer (5.90 × 1010 s-1) in the molecular pentad. Since the electron transfer from the singlet ZnPc to BODIPY is thermodynamically not feasible, the singlet ZnPc decayed to populates the triplet ZnPc , in addition to the grounds state. These findings suggest the potential of the examined ZnPc -BODIPY pentad to be efficient photosynthetic antenna in the artificial photosynthetic systems.


2006 ◽  
Vol 110 (50) ◽  
pp. 25411-25420 ◽  
Author(s):  
Rodrigo E. Palacios ◽  
Gerdenis Kodis ◽  
Christian Herrero ◽  
Ernesto Mariño Ochoa ◽  
Miguel Gervaldo ◽  
...  

2013 ◽  
Vol 41 ◽  
pp. 08010
Author(s):  
M. Maiuri ◽  
J.J. Snellenburg ◽  
I.H.M. van Stokkum ◽  
S. Pillai ◽  
D. Gust ◽  
...  

2002 ◽  
Vol 106 (10) ◽  
pp. 2036-2048 ◽  
Author(s):  
Gerdenis Kodis ◽  
Paul A. Liddell ◽  
Linda de la Garza ◽  
P. Christian Clausen ◽  
Jonathan S. Lindsey ◽  
...  

2005 ◽  
Vol 77 (6) ◽  
pp. 1001-1008 ◽  
Author(s):  
Rodrigo E. Palacios ◽  
Stephanie L. Gould ◽  
Christian Herrero ◽  
Michael Hambourger ◽  
Alicia Brune ◽  
...  

Artificial photosynthetic antenna systems have been synthesized based on carotenoid polyenes and polymer-polyenes covalently attached to tetrapyrroles. Absorption of light in the blue/green region of the spectra excites the polyenes to their S2 state, and ultrafast singlet energy transfer to the tetrapyrroles occurs when the chromophores are in partial conjugation. The additional participation of other excited states of the polyene in the energy-transfer process is a requirement for perfect antenna function. Analogs of photosynthetic reaction centers consisting of tetrapyrrole chromophores covalently linked to electron acceptors and donors have been prepared. Excitation of these constructs results in a cascade of energy transfer/electron transfer which, in selected cases, forms a final charge-separated state characterized by a giant dipole moment (>150 D), a quantum yield approaching unity, a significant fraction of the photon energy stored as chemical potential, and a lifetime sufficient for reaction with secondary electron donors and acceptors. A new antenna-reaction center complex is described in which a carotenoid moiety is located in partial conjugation with the tetrapyrrole π-system allowing fast energy transfer (<100 fs) between the chromophores. In this assembly, the energy transduction process can be initiated by light absorbed by the polyene.


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